Intermetallics are atomically ordered crystalline compounds containing two or more main group and transition metals. In addition to their rich crystal chemistry, intermetallics display unique properties of interest for a variety of applications, including superconductivity, hydrogen storage, and catalysis. Because of the presence of metals with a wide range of reduction potentials, the controlled synthesis of intermetallics can be difficult. Recently, soft chemical syntheses such as the modified polyol and ship-in-a-bottle methods have helped advance the preparation of these materials. However, phase-segregated products and complex multistep syntheses remain common. Here, we demonstrate the use of heterobimetallic single-source precursors for the synthesis of 10–15 and 11–15 binary intermetallics. The coordination environment of the precursor, as well as the exact temperature used play a critical role in determining the crystalline intermetallic phase that is produced, highlighting the potential versatility of this approach in the synthesis of a variety of compounds. Furthermore, we show that a recently developed novel plasma-processing technique is successful in removing the surface graphitic carbon observed in some of the prepared compounds. This new single-source precursor approach is a powerful addition to the synthesis of atomically ordered intermetallic compounds and will help facilitate their further study and development for future applications.